We present results of our investigations on nickel silicidation of top-down fabricated silicon nanowires (SiNWs). Control over the silicidation process is important for the application of SiNWs in reconfigurable field-effect transistors. Silicidation is performed using a rapid thermal annealing process on the SiNWs fabricated by electron beam lithography and inductively-coupled plasma etching. The effects of variations in crystallographic orientations of SiNWs and different NW designs on the silicidation process are studied. Scanning electron microscopy and transmission electron microscopy are performed to study Ni diffusion, silicide phases, and silicide–silicon interfaces. Control over the silicide phase is achieved together with atomically sharp silicide–silicon interfaces. We find that {111} interfaces are predominantly formed, which are energetically most favorable according to density functional theory calculations. However, control over the silicide length remains a challenge.